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Title: The effect of ion irradiation on the dissolution of UO 2 and UO 2 -based simulant fuel

Abstract

Our aim is to study the separate effect of fission fragment damage on the dissolution of simulant UK advanced gas-cooled reactor nuclear fuel in water. Plain UO 2 and UO 2 samples, doped with inactive fission products to simulate 43 GWd/tU of burn-up, were fabricated. A set of these samples were then irradiated with 92 MeV 129Xe 23+ ions to a fluence of 4.8 × 10 15 ions/cm 2 to simulate the fission damage that occurs within nuclear fuels. The primary effect of the irradiation on the UO 2 samples, observed by scanning electron microscopy, was to induce a smoothening of the surface features and formation of hollow blisters, which was attributed to multiple overlap of ion tracks. Dissolution experiments were conducted in single-pass flow-through (SPFT) mode under anoxic conditions (<0.1 O 2 ppm in Ar) to study the effect of the induced irradiation damage on the dissolution of the UO 2 matrix with data collection capturing six minute intervals for several hours. These time-resolved data showed that the irradiated samples showed a higher initial release of uranium than unirradiated samples, but that the uranium concentrations converged towards ~10 -9 mol/l after a few hours. And apart from the initialmore » spike in uranium concentration, attributed to irradiation induced surficial micro-structural changes, no noticeable difference in uranium chemistry as measured by X-ray electron spectroscopy or ‘effective solubility’ was observed between the irradiated, doped and undoped samples in this work. Some secondary phase formation was observed on the surface of UO 2 samples after the dissolution experiment.« less

Authors:
ORCiD logo [1];  [2];  [2]; ORCiD logo [2];  [3];  [4];  [4];  [3];  [2];  [5]
  1. Univ. of Cambridge (United Kingdom). Dept. of Earth Sciences; Imperial College, London (United Kingdom). Dept. of Materials
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  4. Univ. of Caen (France). Center for Research on Ions, Materials and Photonics (CIMAP)
  5. Univ. of Cambridge (United Kingdom). Dept. of Earth Sciences
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1413473
Report Number(s):
PNNL-SA-129551
Journal ID: ISSN 0925-8388; PII: S092583881733997X; TRN: US1800437
Grant/Contract Number:
AC0576RL01830
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Alloys and Compounds
Additional Journal Information:
Journal Volume: 735; Journal Issue: C; Journal ID: ISSN 0925-8388
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; UO2; simfuel; ion irradiation; radiation damage; dissolution; secondary phases

Citation Formats

Popel, Aleksej J., Wietsma, Thomas W., Engelhard, Mark H., Lea, Alan S., Qafoku, Odeta, Grygiel, Clara, Monnet, Isabelle, Ilton, Eugene S., Bowden, Mark E., and Farnan, Ian. The effect of ion irradiation on the dissolution of UO 2 and UO 2 -based simulant fuel. United States: N. p., 2017. Web. doi:10.1016/J.JALLCOM.2017.11.216.
Popel, Aleksej J., Wietsma, Thomas W., Engelhard, Mark H., Lea, Alan S., Qafoku, Odeta, Grygiel, Clara, Monnet, Isabelle, Ilton, Eugene S., Bowden, Mark E., & Farnan, Ian. The effect of ion irradiation on the dissolution of UO 2 and UO 2 -based simulant fuel. United States. doi:10.1016/J.JALLCOM.2017.11.216.
Popel, Aleksej J., Wietsma, Thomas W., Engelhard, Mark H., Lea, Alan S., Qafoku, Odeta, Grygiel, Clara, Monnet, Isabelle, Ilton, Eugene S., Bowden, Mark E., and Farnan, Ian. Tue . "The effect of ion irradiation on the dissolution of UO 2 and UO 2 -based simulant fuel". United States. doi:10.1016/J.JALLCOM.2017.11.216.
@article{osti_1413473,
title = {The effect of ion irradiation on the dissolution of UO 2 and UO 2 -based simulant fuel},
author = {Popel, Aleksej J. and Wietsma, Thomas W. and Engelhard, Mark H. and Lea, Alan S. and Qafoku, Odeta and Grygiel, Clara and Monnet, Isabelle and Ilton, Eugene S. and Bowden, Mark E. and Farnan, Ian},
abstractNote = {Our aim is to study the separate effect of fission fragment damage on the dissolution of simulant UK advanced gas-cooled reactor nuclear fuel in water. Plain UO2 and UO2 samples, doped with inactive fission products to simulate 43 GWd/tU of burn-up, were fabricated. A set of these samples were then irradiated with 92 MeV 129Xe23+ ions to a fluence of 4.8 × 1015 ions/cm2 to simulate the fission damage that occurs within nuclear fuels. The primary effect of the irradiation on the UO2 samples, observed by scanning electron microscopy, was to induce a smoothening of the surface features and formation of hollow blisters, which was attributed to multiple overlap of ion tracks. Dissolution experiments were conducted in single-pass flow-through (SPFT) mode under anoxic conditions (<0.1 O2 ppm in Ar) to study the effect of the induced irradiation damage on the dissolution of the UO2 matrix with data collection capturing six minute intervals for several hours. These time-resolved data showed that the irradiated samples showed a higher initial release of uranium than unirradiated samples, but that the uranium concentrations converged towards ~10-9 mol/l after a few hours. And apart from the initial spike in uranium concentration, attributed to irradiation induced surficial micro-structural changes, no noticeable difference in uranium chemistry as measured by X-ray electron spectroscopy or ‘effective solubility’ was observed between the irradiated, doped and undoped samples in this work. Some secondary phase formation was observed on the surface of UO2 samples after the dissolution experiment.},
doi = {10.1016/J.JALLCOM.2017.11.216},
journal = {Journal of Alloys and Compounds},
number = C,
volume = 735,
place = {United States},
year = {Tue Nov 21 00:00:00 EST 2017},
month = {Tue Nov 21 00:00:00 EST 2017}
}

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